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Highly Efficient Photo-Induced Charge Separation enabled by Metal-Chalcogenide Interfaces in Quantum-Dot/Metal-Oxide Hybrid Phototransistors

DOI:10.1021/acsami.0c01176 期刊:ACS Applied Materials & Interfaces 出版年份:2020 更新时间:2025-09-23 15:19:57
摘要: Quantum dot (QD)-based optoelectronics have received a large amount of interest for the versatile applications due to their excellent photosensitivity, facile solution processability, and the wide range of band gap tunability. In addition, the QD-based hybrid devices which are combined with various high-mobility semiconductors have been actively researched to enhance the optoelectronic characteristics as well as maximize the zero-dimensional structural advantages, such as tunable band gap and high light absorption. However, the difficulty of highly efficient charge transfer between QDs and the semiconductors, and the lack of systematic analysis for the interfaces have impeded the fidelity of this platform, resulting in complex device architectures and unsatisfactory device performance. Here, we report ultra-high detective phototransistors with highly efficient photo-induced charge separation using Sn2S6 4--capped CdSe QD/amorphous oxide semiconductor (AOS) hybrid structure. The photo-induced electron transfer characteristics at the interface of the two materials were comprehensively investigated with an array of electrochemical and spectroscopic analysis. In particular, the photocurrent imaging microscopy revealed that interface engineering in QD-AOS with chelating chalcometallate ligands cause efficient charge transfer, resulting in photovoltaic-dominated responses over whole channel area. On the other hands, monodentate ligands incorporated QD-AOS based devices typically exhibit limited charge transfer with atomic vibration, showing photo-thermoelectric-dominated responses in the drain electrode area.
作者: Jaehyun Kim,Sung Min Kwon,Chanho Jo,Jae-Sang Heo,Won Bin Kim,Hyun Suk Jung,Yong-Hoon Kim,Myung-Gil Kim,Sung Kyu Park
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Investigating the charge transfer properties of CdSe QDs/a-IGZO hybrid phototransistors in conjunction with surface structures of QDs capped with various ligands to achieve highly efficient photo-induced charge separation.

The research demonstrated that chelating chalcometallate ligands (Sn2S6 4-) offer a facile route to realize unprecedentedly high performance QD-based hybrid phototransistors with marginal complexity, providing compatibility with large-scaled applications and on-chip scaled devices. The Sn2S6 4--capped phototransistors showed photovoltaic-dominated response behaviors due to lower density of trap sites on QD surface, exhibiting high photosensitivity, EQE, dynamic range, and fast response time.

The study acknowledges the difficulty in achieving highly efficient charge transfer between QDs and semiconductors and the lack of systematic analysis for the interfaces, which can lead to complex device architectures and unsatisfactory device performance.

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